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Xinhua Xie

Publications and source records attributed to Xinhua Xie.

26 records · Page 2Linked to original sources

Direct Observation of Molecular Oxygen Production from Carbon Dioxide

Oxygen ($O_2$) is one of the most important elements required to sustain life. The concentration of $O_2$ on Earth has been accumulated over millions of years and has a direct connection with that of $CO_2$. Further, $CO_2$ plays an important role in many other planetary atmospheres. Therefore, molecular reactions involving $CO_2$ are critical for studying the atmospheres of such planets. Existing studies on the dissociation of $CO_2$ are exclusively focused on the C--O bond breakage. Here we report first experiments on the direct observation of molecular Oxygen formation from $CO_2$ in strong laser fields with a reaction microscope. Our accompanying simulations suggest that $CO_2$ molecules may undergo bending motion during and after strong-field ionization which supports the molecular Oxygen formation process. The observation of the molecular Oxygen formation from $CO_2$ may trigger further experimental and theoretical studies on such processes with laser pulses, and provide hints in studies of the $O_2$ and $CO_2^+$ abundance in $CO_2$-dominated planetary atmospheres.

physics.chem-ph↗

Coincidence spectroscopy of high-lying Rydberg states produced in strong laser fields

We report on the measurement of electron emission after the interaction of strong laser pulses with atoms and molecules. These electrons originate from high-lying Rydberg states with quantum numbers up to $n \lesssim 120$ formed by frustrated field ionization. Simulations show that both tunneling ionization by a weak dc field and photoionization by the black-body radiation contribute to delayed electron emission on the nano- to microsecond scale. We measured ionization rates from these Rydberg states by coincidence spectroscopy. Further, the dependence of the Rydberg-state production on the ellipticity of the driving laser field proves that such high-lying Rydberg states are populated through electron recapture. The present experiment provides detailed quantitative information on Rydberg production by frustrated field ionization.

physics.atom-ph↗

Fragmentation of long-lived hydrocarbons after strong field ionization

We experimentally and theoretically investigated the deprotonation process on nanosecond to microsecond timescale in ethylene and acetylene molecules, following their double ionization by a strong femtosecond laser field. In our experiments we utilized coincidence detection with the reaction microscope technique, and found that both the lifetime of the long-lived ethylene dication leading to the delayed deprotonation and the relative channel strength of the delayed deprotonation compared to the prompt one have no evident dependence on the laser pulse duration and the laser peak intensity. Quantum chemical simulations suggest that such delayed fragmentation originates from the tunneling of near-dissociation-threshold vibrational states through a dissociation barrier on a dication electronic state along C--H stretching. Such vibrational states can be populated through strong field double ionization induced vibrational excitation on an electronically excited state in the case of ethylene, and through intersystem crossing from electronically excited states to the electronic ground state in the case of acetylene.

physics.chem-ph↗

Real-time probing electron dynamics of an atom in a strong infrared laser field

We present theoretical studies on real-time probing the electron density evolution of an atom in a strong infrared (IR) laser field with few-cycle near-infrared (NIR) and attosecond extreme-ultraviolet (XUV) pulses. Our results indicate that the electron density near the tunneling barrier is reflected in the additional tunneling ionization yield with a delayed NIR pulse and the electron density near the nucleus can be probed by the single photoionization yield with a delayed XUV pulse. It turns out the NIR-probing scheme can be used to study the polarization of the system in an external IR field and the XUV-probing can be additionally applied to explore excitation dynamics during and after the IR field interaction.

physics.atom-ph↗

Two-Dimensional Attosecond Electron Wave Packet Interferometry

We propose a two-dimensional interferometry based on electron wave packet interference with a cycle-shaped orthogonally polarized two-color laser field. With such method, sub-cycle and inter-cycle interferences can be disentangled into different direction in the measured photoelectron momentum spectra. With the cycle-shaped laser field, the Coulomb influence can be minimized and the overlapping of interference fringes with the complicate low-energy structures can be avoided as well. The contributions of excitation effect and long-range Coulomb potential can be traced in the Fourier domain of the photoelectron distributions. With these advantages, it allows to get precise information on valence electron dynamics of atoms or molecules with attosecond resolution and additional spatial information with angstrom resolution.

physics.atom-ph↗

Laser-sub-cycle two-dimensional electron momentum mapping using orthogonal two-color fields

The two-dimensional sub-cycle-time to electron momentum mapping provided by orthogonal two-color laser fields is applied to photoelectron spectroscopy. Using neon as the example we gain experimental access to the dynamics of emitted electron wave packets in electron momenta spectra measured by coincidence momentum imaging. We demonstrate the opportunities provided by this time-to-momentum mapping by investigating the influence of the parent ion on the emitted electrons on laser-sub-cycle times. It is found that depending on their sub-cycle birth time the trajectories of photoelectrons are affected differently by the ion's Coulomb field.

physics.atom-ph↗

Signature of multi-channel interference in high-order harmonic generation from N2 driven by intense mid-infrared pulses

We investigate the multi-electron dynamics in high-order harmonic generation (HHG) from N2 molecules. Clear spectral minima are observed in the cutoff region at all three mid-infrared wavelengths (i.e., 1300, 1400 and 1500 nm) chosen in our experiment. It is found that the positions of the spectral minima do not depend on the alignment angles of molecules. In addition, the spectral minima shift almost linearly with the increasing laser intensity at all three wavelengths, which provides a strong evidence on the dynamic multi-channel interference origin of these minima. The advantages of observation of dynamic multi-channel interference based on HHG driven by long wavelength lasers are discussed.

physics.atom-ph↗

Attosecond-recollision-controlled selective fragmentation of polyatomic molecules

Control over various fragmentation reactions of a series of polyatomic molecules (acetylene, ethylene, 1,3-butadiene) by the optical waveform of intense few-cycle laser pulses is demonstrated experimentally. We show both experimentally and theoretically that the responsible mechanism is inelastic ionization from inner-valence molecular orbitals by recolliding electron wavepackets, whose recollision energy in few-cycle ionizing laser pulses strongly depends on the optical waveform. Our work demonstrates an efficient and selective way of pre-determining fragmentation and isomerization reactions in polyatomic molecules on sub-femtosecond time-scales.

physics.chem-ph↗